The Limits of Inelastic Tunneling Spectroscopy for Identifying Transport Pathways

Abstract

Inelastic electron tunneling spectroscopy (IETS) is a powerful tool to study the properties of molecular junctions. In particular, it is considered useful for extracting information on electron transport pathways. We explore the limits of this approach by comparing computed interatomic transmission pathways with IETS intensities for different molecular junctions, employing a new efficient implementation for evaluating IETS intensities via the mode-tracking algorithm. While we indeed find a correlation between pathways and IETS intensities when vibrations are clearly localized on atoms off the transport pathway, we do not see such a correlation for molecules with less localized vibrations, even if transport pathways only a sample part of the molecule and even if a statistical analysis over the vibrational modes is made. This could indicate that the significance of IETS signals for transport pathways is limited to molecules with localized vibrational modes.

How Surface Defects Shape the Excitons and Photoluminescence of Ultrasmall CdSe Quantum Dots

“…In the SCIS calculations, we further employed the Penn model for the description of the dielectric response function. 26 The local Loẅdin populations 27,29 for MOs and excitonic holes, the IPR values, 28 the electric dipole moments, 47 and the DCs were implemented in a local version of the ARTAIOS program package 48 which was used in the calculations, respectively.…”